Preheat oven to 350°F. Spray a 9-inch pie pan with non-stick cooking spray and set aside.
Make the crust: In a large bowl, stir together 2/3 cup sweetened condensed milk, 1 large egg white, 1 1/2 teaspoons vanilla, and 1/8 teaspoon salt until combined.
Add 3 1/2 cups sweetened coconut to the wet mixture and stir until the coconut is evenly moistened.
Press the coconut mixture firmly and evenly into the prepared pie pan, pressing it up the sides to form a crust.
Bake the crust for 10–12 minutes, until lightly golden. Remove from the oven and let the crust cool until it is warm or room temperature.
While the crust cools, make the filling: In a medium bowl, whisk together the 114-ounce can sweetened condensed milk and 4 large egg yolks until smooth. Whisk in the zest of 1 large lime and 1/2 cup lime juice until fully combined.
Pour the filling over the cooled coconut macaroon crust and smooth the top. Return the pie to the oven and bake for 15–17 minutes, or until the filling is set (center should not be liquid) and the coconut crust is golden brown around the edges.
Remove the pie from the oven and cool on a wire rack to room temperature, then chill in the refrigerator for at least 1 hour to allow the filling to fully set before serving. If you prefer, you may use regular limes or bottled key lime juice in place of key limes.